Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries

Dusan Strmcnik; Ivano E. Castelli; Justin G. Connell; Dominik Haering; Milena Zorko; Pedro Martins; Pietro P. Lopes; Bostjan Genorio; Thomas Østergaard; Hubert A. Gasteiger; Filippo Maglia; Byron K. Antonopoulos; Vojislav R. Stamenkovic; Jan Rossmeisl; Nenad M. Markovic

doi:10.1038/s41929-018-0047-z

Electrocatalytic transformation of HF impurity to H₂ and LiF in lithium-ion batteries

Dusan Strmcnik, Ivano E. Castelli, Justin G. Connell, Dominik Haering, Milena Zorko, Pedro Martins, Pietro P. Lopes, Bostjan Genorio, Thomas Østergaard, Hubert A. Gasteiger, Filippo Maglia, Byron K. Antonopoulos, Vojislav R. Stamenkovic, Jan Rossmeisl, Nenad M. Markovic

Chair of Technical Electrochemistry

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142 Scopus citations

Abstract

The formation of solid electrolyte interphase on graphite anodes plays a key role in the efficiency of Li-ion batteries. However, to date, fundamental understanding of the formation of LiF as one of the main solid electrolyte interphase components in hexafluorophosphate-based electrolytes remains elusive. Here, we present experimental and theoretical evidence that LiF formation is an electrocatalytic process that is controlled by the electrochemical transformation of HF impurity to LiF and H₂. Although the kinetics of HF dissociation and the concomitant production of LiF and H₂ is dependent on the structure and nature of surface atoms, the underlying electrochemistry is the same. The morphology, and thus the role, of the LiF formed is strongly dependent on the nature of the substrate and HF inventory, leading to either complete or partial passivation of the interface. Our finding is of general importance and may lead to new opportunities for the improvement of existing, and design of new, Li-ion technologies.

Original language	English
Pages (from-to)	255-262
Number of pages	8
Journal	Nature Catalysis
Volume	1
Issue number	4
DOIs	https://doi.org/10.1038/s41929-018-0047-z
State	Published - 1 Apr 2018

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Strmcnik, D., Castelli, I. E., Connell, J. G., Haering, D., Zorko, M., Martins, P., Lopes, P. P., Genorio, B., Østergaard, T., Gasteiger, H. A., Maglia, F., Antonopoulos, B. K., Stamenkovic, V. R., Rossmeisl, J., & Markovic, N. M. (2018). Electrocatalytic transformation of HF impurity to H₂ and LiF in lithium-ion batteries. Nature Catalysis, 1(4), 255-262. https://doi.org/10.1038/s41929-018-0047-z

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title = "Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries",

abstract = "The formation of solid electrolyte interphase on graphite anodes plays a key role in the efficiency of Li-ion batteries. However, to date, fundamental understanding of the formation of LiF as one of the main solid electrolyte interphase components in hexafluorophosphate-based electrolytes remains elusive. Here, we present experimental and theoretical evidence that LiF formation is an electrocatalytic process that is controlled by the electrochemical transformation of HF impurity to LiF and H2. Although the kinetics of HF dissociation and the concomitant production of LiF and H2 is dependent on the structure and nature of surface atoms, the underlying electrochemistry is the same. The morphology, and thus the role, of the LiF formed is strongly dependent on the nature of the substrate and HF inventory, leading to either complete or partial passivation of the interface. Our finding is of general importance and may lead to new opportunities for the improvement of existing, and design of new, Li-ion technologies.",

author = "Dusan Strmcnik and Castelli, {Ivano E.} and Connell, {Justin G.} and Dominik Haering and Milena Zorko and Pedro Martins and Lopes, {Pietro P.} and Bostjan Genorio and Thomas {\O}stergaard and Gasteiger, {Hubert A.} and Filippo Maglia and Antonopoulos, {Byron K.} and Stamenkovic, {Vojislav R.} and Jan Rossmeisl and Markovic, {Nenad M.}",

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doi = "10.1038/s41929-018-0047-z",

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Strmcnik, D, Castelli, IE, Connell, JG, Haering, D, Zorko, M, Martins, P, Lopes, PP, Genorio, B, Østergaard, T, Gasteiger, HA, Maglia, F, Antonopoulos, BK, Stamenkovic, VR, Rossmeisl, J & Markovic, NM 2018, 'Electrocatalytic transformation of HF impurity to H₂ and LiF in lithium-ion batteries', Nature Catalysis, vol. 1, no. 4, pp. 255-262. https://doi.org/10.1038/s41929-018-0047-z

TY - JOUR

T1 - Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries

AU - Strmcnik, Dusan

AU - Castelli, Ivano E.

AU - Connell, Justin G.

AU - Haering, Dominik

AU - Zorko, Milena

AU - Martins, Pedro

AU - Lopes, Pietro P.

AU - Genorio, Bostjan

AU - Østergaard, Thomas

AU - Gasteiger, Hubert A.

AU - Maglia, Filippo

AU - Antonopoulos, Byron K.

AU - Stamenkovic, Vojislav R.

AU - Rossmeisl, Jan

AU - Markovic, Nenad M.

PY - 2018/4/1

Y1 - 2018/4/1

N2 - The formation of solid electrolyte interphase on graphite anodes plays a key role in the efficiency of Li-ion batteries. However, to date, fundamental understanding of the formation of LiF as one of the main solid electrolyte interphase components in hexafluorophosphate-based electrolytes remains elusive. Here, we present experimental and theoretical evidence that LiF formation is an electrocatalytic process that is controlled by the electrochemical transformation of HF impurity to LiF and H2. Although the kinetics of HF dissociation and the concomitant production of LiF and H2 is dependent on the structure and nature of surface atoms, the underlying electrochemistry is the same. The morphology, and thus the role, of the LiF formed is strongly dependent on the nature of the substrate and HF inventory, leading to either complete or partial passivation of the interface. Our finding is of general importance and may lead to new opportunities for the improvement of existing, and design of new, Li-ion technologies.

AB - The formation of solid electrolyte interphase on graphite anodes plays a key role in the efficiency of Li-ion batteries. However, to date, fundamental understanding of the formation of LiF as one of the main solid electrolyte interphase components in hexafluorophosphate-based electrolytes remains elusive. Here, we present experimental and theoretical evidence that LiF formation is an electrocatalytic process that is controlled by the electrochemical transformation of HF impurity to LiF and H2. Although the kinetics of HF dissociation and the concomitant production of LiF and H2 is dependent on the structure and nature of surface atoms, the underlying electrochemistry is the same. The morphology, and thus the role, of the LiF formed is strongly dependent on the nature of the substrate and HF inventory, leading to either complete or partial passivation of the interface. Our finding is of general importance and may lead to new opportunities for the improvement of existing, and design of new, Li-ion technologies.

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EP - 262

JO - Nature Catalysis

JF - Nature Catalysis

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ER -

Electrocatalytic transformation of HF impurity to H₂ and LiF in lithium-ion batteries

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